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  1. Mechanocatalytic Hydrogenolysis of the Lignin Model Dimer Benzyl Phenyl Ether over Supported Palladium Catalysts

    This work demonstrates the mechanocatalytic hydrogenolysis of the ether bond in the lignin model compound benzyl phenyl ether (BPE) and hardwood lignin isolated by hydrolysis with supercritical water. Pd catalysts with 4 wt % loading on Al2O3 and SiO2 supports achieve 100% conversion of BPE with a toluene production rate of (2.6–2.9) × 10–5 mol·min–1. The formation of palladium hydrides under H2 gas flow contributes to an increase in the turnover frequency by a factor of up to 300 compared to Ni on silica–alumina. While a near-quantitative toluene yield is obtained, some of the phenolic products remain adsorbed on themore » catalyst.« less
  2. Ionomer-free and recyclable porous-transport electrode for high-performing proton-exchange-membrane water electrolysis

    Abstract Clean hydrogen production requires large-scale deployment of water-electrolysis technologies, particularly proton-exchange-membrane water electrolyzers (PEMWEs). However, as iridium-based electrocatalysts remain the only practical option for PEMWEs, their low abundance will become a bottleneck for a sustainable hydrogen economy. Herein, we propose high-performing and durable ionomer-free porous transport electrodes (PTEs) with facile recycling features enabling Ir thrifting and reclamation. The ionomer-free porous transport electrodes offer a practical pathway to investigate the role of ionomer in the catalyst layer and, from microelectrode measurements, point to an ionomer poisoning effect for the oxygen evolution reaction. The ionomer-free porous transport electrodes demonstrate a voltagemore » reduction of > 600 mV compared to conventional ionomer-coated porous transport electrodes at 1.8 A cm −2 and <0.1 mg Ir cm −2 , and a voltage degradation of 29 mV at average rate of 0.58 mV per 1000-cycles after 50k cycles of accelerated-stress tests at 4 A cm −2 . Moreover, the ionomer-free feature enables facile recycling of multiple components of PEMWEs, which is critical to a circular clean hydrogen economy.« less
  3. Design and operating principles for high-performing anion exchange membrane water electrolyzers

    Anion-exchange-membrane water electrolyzers (AEMWEs) provide a promising pathway to utilize low-carbon renewable electricity to produce clean hydrogen at high efficiency and purity, while maintaining low system costs compared to incumbent technologies. Though significant progress has been made in developing membranes and catalysts, AEMWEs still require better performance and durability to realize widespread deployment. Here, we overcome these challenges by decoupling anode and cathode polarization behavior via integration of a reference electrode in the membrane-electrode assembly. This measurement identified that the mass-transport losses dominate the cathode overpotential if feeding with electrolytes, while kinetic losses dominate the anode overpotential. These losses aremore » mitigated by varying electrode properties and operating strategies, where a more hydrophobic, optimal loaded cathode, a high porosity anode, and operating with the cathode dry exhibited the best performance. These findings eventually enabled achieving a high-performing and durable complete PGM-free AEMWE operating at 1.5 Acm–2 for over 500h with negligible degradation, demonstrating significant progress for AEMWEs.« less

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